Preparation of electrochemically exfoliated graphene sheets using DC switching voltages

  • Sungmook Lim
  • Jong Hun Han
  • Hyun Wook Kang
  • Jea Uk LeeEmail author
  • Wonoh LeeEmail author
Original Article


Among various methods to produce graphene sheets, electrochemical exfoliation has been regarded as an effective method for the mass production of high-quality graphene sheets because of its simplicity and environmental friendliness. However, conventional electrochemical exfoliation has a disadvantage of accumulating intercalating ions at graphite interlayers owing to the use of a constant voltage. In this study, we developed a DC switching technique to achieve more efficient intercalation of ions than that in the conventional method. In the DC switching method, positive and negative voltages are successively applied to release the accumulated intercalating ions. By testing various conditions, we found the optimum switching time to produce high-quality graphene sheets with the highest yield rate and the highest electrical conductivity. As a result, the graphene sheets using this DC switching technique showed 85% higher yield rate, 193% higher electrical conductivity, 160% larger area, and 25% thinner thickness than those obtained when using a constant DC method. We believe that this DC switching technique can be used for large-scale production of high-quality graphene sheets.


Graphene Electrochemical exfoliation DC switching technique Intercalating ions Electrical conductivity 



This work was supported by the National Research Foundation (NRF) of Korea grant funded by the Ministry of Science, ICT and Future Planning (2016M3A7B4021149 and 2018R1A2A2A15020973). Also, the authors are grateful to the Center for Research Facilities at the Chonnam National University for the assistance in chemical analyses (AFM, Raman and XPS).

Compliance with ethical standards

Conflict of interest

No potential conflict of interest relevant to this article is reported.


  1. 1.
    Paek SM, Yoo E, Honma I (2009) Enhanced cyclic performance and lithium storage capacity of SnO2/graphene nanoporous electrodes with three-dimensionally delaminated flexible structure. Nano Lett 1:72. CrossRefGoogle Scholar
  2. 2.
    Hsieh CT, Yang BH, Lin JY (2011) One- and two-dimensional carbon nanomaterials as counter electrodes for dye-sensitized solar cells. Carbon 49:3092. CrossRefGoogle Scholar
  3. 3.
    Stoller MD, Park S, Zhu Y, An J, Rouff RS (2008) Graphene-based ultracapacitors. Nano Lett 10:3498. CrossRefGoogle Scholar
  4. 4.
    Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV, Grigorieva IV, Frisov AA (2004) Electric field effect in atomically thin carbon films. Science 306:666. CrossRefGoogle Scholar
  5. 5.
    Nair RR, Blake P, Grigorenko AN, Novoselov KS, Booth TJ, Stauber T, Peres NMR, Geim AK (2008) Fine structure constant defines visual transparency of graphene. Science 320:1308. CrossRefGoogle Scholar
  6. 6.
    Lee C, Wei XD, Kysar JW, Hone J (2008) Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321:385. CrossRefGoogle Scholar
  7. 7.
    Na Y, Song YI, Kim SW, Suh SJ (2017) Study on properties of eco-friendly reduction agents for the reduced graphene oxide method. Carbon Lett 24:1. CrossRefGoogle Scholar
  8. 8.
    Lee W, Oh Y, Lee KE, Lee JU (2015) Contrast enhancement for quantitative image analysis of graphene oxide using optical microscopy for Si-based field effect transistors. Mater Sci Semicon Process 39:521. CrossRefGoogle Scholar
  9. 9.
    Kwon YJ, Kim Y, Jeon H, Cho S, Lee W, Lee JU (2017) Graphene/carbon nanotube hybrid as a multi-functional interfacial reinforcement for carbon fiber-reinforced composites. Compos Pt B Eng 122:23. CrossRefGoogle Scholar
  10. 10.
    Luan VH, Bae D, Han JH, Lee W (2018) Mussel-inspired dopamine-mediated graphene hybrid with silver nanoparticles for high performance electrochemical energy storage electrodes. Compos Pt B Eng 134:141. CrossRefGoogle Scholar
  11. 11.
    Zhong YL, Tian Z, Simon GP, Li D (2014) Scalable production of graphene via wet chemistry: progress and challenges. Mater Today 18:73. CrossRefGoogle Scholar
  12. 12.
    Wang J, Manga KK, Bao Q, Loh KP (2011) High-yield synthesis of few-layer graphene flakes through electrochemical expansion of graphite in propylene carbonate electrolyte. J Am Chem Soc 23:8888. CrossRefGoogle Scholar
  13. 13.
    Yu P, Lowe SE, Simon GP, Zhong YL (2015) Electrochemical exfoliation of graphite and production of functional graphene. Curr Opin Colloid Interface Sci 20:329. CrossRefGoogle Scholar
  14. 14.
    Hsieh CT, Hsueh JH (2016) Electrochemical exfoliation of graphene sheets from a natural graphite flask in the presence of sulfate ions at different temperatures. RSC Adv 6:64826. CrossRefGoogle Scholar
  15. 15.
    Parvez K, Li R, Puniredd SR, Hernandez Y, Hinkel F, Wang S, Feng X, Mullen K (2013) Electrochemically exfoliated graphene as solution-processable, highly conductive electrodes for organic electronics. ACS Nano 7:3598. CrossRefGoogle Scholar
  16. 16.
    Su CY, Lu AY, Xu Y, Chen FR, Khlobystov AN, Li LJ (2011) High-quality thin graphene films from fast electrochemical exfoliation. ACS Nano 5:2332. CrossRefGoogle Scholar
  17. 17.
    Ferrari AC, Meyer JC, Scardaci V, Casiraghi C, Lazzeri M, Mauri F, Piscanec S, Jiang D, Novoselov S, Roth S, Geim AK (2006) Raman spectrum of graphene and graphene layers. Phys Rev Lett 97:187401. CrossRefGoogle Scholar
  18. 18.
    Lopez V, Sundaram RS, Navarro CG, Olea D, Burghard M, Herrero JG, Zamora F, Kern K (2009) Chemical vapor deposition of graphene oxide: a route to highly-conductive graphene monolayers. Adv Mater 21:4683. CrossRefGoogle Scholar
  19. 19.
    Krauss B, Lohmann T, Chae DH, Haluska M, Klitzing KV, Smet JH (2009) Laser-induced disassembly of a graphene single crystal into a nanocrystalline network. Phys Rev B 79:165428. CrossRefGoogle Scholar
  20. 20.
    Evlashin SA, Svyakhovskiy SE, Fedorov FS, Mankelevich YA, Dyakonov PV, Minaev NV, Dagesyan SA, Maslakov KI, Khmelnitsky RA, Suetin NV, Akhatov IS, Nasibulin AG (2018) Ambient condition production of high quality reduced graphene oxide. Adv Mater Interf 5:1800737. CrossRefGoogle Scholar
  21. 21.
    Park S, Rouff RS (2010) Chemical methods for production of graphenes. Nat Nanotechnol 4:217. CrossRefGoogle Scholar
  22. 22.
    Compton OC, Jain B, Dikin DA, Abouimrane A, Amine K, Nguyen ST (2011) Chemically active reduced graphene oxide with tunable C/O ratios. ACS Nano 5:4380. CrossRefGoogle Scholar
  23. 23.
    Parvez K, Wu ZS, Li R, Liu X, Graf R, Wang S, Feng X, Mullen K (2014) Exfoliation of graphite into graphene in aqueous solutions of inorganic salts. J Am Chem Soc 136:6083. CrossRefGoogle Scholar
  24. 24.
    Kwon YJ, Kwon Y, Park HS, Lee JU (2019) Mass-produced electrochemically exfoliated graphene for ultrahigh thermally conductive paper using a multimetal electrode system. Adv Mater Interf 6:1900095. CrossRefGoogle Scholar
  25. 25.
    Chen CH, Yang SW, Chuang MC, Woon WY, Su CY (2015) Towards the continuous production of high crystallinity graphene via electrochemical exfoliation with molecular in situ encapsulation. Nanoscale 7:15362. CrossRefGoogle Scholar
  26. 26.
    Abdelkader AM, Kinloch IA, Dryfe RAW (2014) Continuous electrochemical exfoliation of micrometer-sized graphene using synergistic ion intercalations and organic solvents. ACS Appl Mater Interfaces 6(3):1632–1639. CrossRefGoogle Scholar

Copyright information

© Korean Carbon Society 2019

Authors and Affiliations

  1. 1.School of Mechanical EngineeringChonnam National UniversityGwangjuRepublic of Korea
  2. 2.School of Chemical EngineeringChonnam National UniversityGwangjuRepublic of Korea
  3. 3.Carbon Industry Frontier Research CenterKorea Research Institute of Chemical Technology (KRICT)DaejonRepublic of Korea

Personalised recommendations